Recent predictions and experimental observations of high Tc superconductivity in hydrogen-rich materials at very high pressures are driving the search for superconductivity in the vicinity of room temperature. We have developed a novel preparation technique that is optimally suited for megabar pressure syntheses of superhydrides using pulsed laser heating while maintaining the integrity of sample-probe contacts for electrical transport measurements to 200 GPa. We detail the synthesis and characterization, including four-probe electrical transport measurements, of lanthanum superhydride samples that display a significant drop in resistivity on cooling beginning around 260 K and pressures of 190 GPa. Additional measurements on two additional samples synthesized the same way show resistance drops beginning as high as 280 K at these pressures. The drop in resistance at these high temperatures is not observed in control experiments on pure La as well as in partially transformed samples at these pressures, and x-ray diffraction as a function of temperature on the superhydride reveal no structural changes on cooling. We suggest that the resistance drop is a signature of the predicted superconductivity in LaH10 near room temperature, in good agreement with density functional structure search and BCS theory calculations. *
Synthesis of well-ordered reduced dimensional carbon solids with extended bonding remains a challenge. For example, few single-crystal organic monomers react under topochemical control to produce single-crystal extended solids. We report a mechanochemical synthesis in which slow compression at room temperature under uniaxial stress can convert polycrystalline or single-crystal benzene monomer into single-crystalline packings of carbon nanothreads, a one-dimensional sp carbon nanomaterial. The long-range order over hundreds of microns of these crystals allows them to readily exfoliate into fibers. The mechanochemical reaction produces macroscopic single crystals despite large dimensional changes caused by the formation of multiple strong, covalent C-C bonds to each monomer and a lack of reactant single-crystal order. Therefore, it appears not to follow a topochemical pathway, but rather one guided by uniaxial stress, to which the nanothreads consistently align. Slow-compression room-temperature synthesis may allow diverse molecular monomers to form single-crystalline packings of polymers, threads, and higher dimensional carbon networks.
Recent theoretical calculations predict that megabar pressure stabilizes very hydrogen-rich simple compounds having new clathrate-like structures and remarkable electronic properties including room-temperature superconductivity. X-ray diffraction and optical studies demonstrate that superhydrides of lanthanum can be synthesized with La atoms in an fcc lattice at 170 GPa upon heating to about 1000 K. The results match the predicted cubic metallic phase of LaH having cages of thirty-two hydrogen atoms surrounding each La atom. Upon decompression, the fcc-based structure undergoes a rhombohedral distortion of the La sublattice. The superhydride phases consist of an atomic hydrogen sublattice with H-H distances of about 1.1 Å, which are close to predictions for solid atomic metallic hydrogen at these pressures. With stability below 200 GPa, the superhydride is thus the closest analogue to solid atomic metallic hydrogen yet to be synthesized and characterized.
Carbon nanothreads are a new one-dimensional sp carbon nanomaterial. They assemble into hexagonal crystals in a room temperature, nontopochemical solid-state reaction induced by slow compression of benzene to 23 GPa. Here we show that pyridine also reacts under compression to form a well-ordered sp product: CNH carbon nitride nanothreads. Solid pyridine has a different crystal structure from solid benzene, so the nontopochemical formation of low-dimensional crystalline solids by slow compression of small aromatics may be a general phenomenon that enables chemical design of properties. The nitrogen in the carbon nitride nanothreads may improve processability, alters photoluminescence, and is predicted to reduce the bandgap.
Compressing glassy carbon above 40 GPa, we have observed a new carbon allotrope with a fully sp 3 -bonded amorphous structure and diamond-like strength. Synchrotron x-ray Raman spectroscopy revealed a continuous pressure-induced sp 2 -to-sp 3 bonding change, while x-ray diffraction confirmed the perseverance of non-crystallinity. The transition was reversible upon releasing pressure. Used as an indenter, the glassy carbon ball demonstrated exceptional strength by reaching 130 GPa with a confining pressure of 60 GPa. Such an extremely large stress difference of >70 GPa has never been observed in any material besides diamond, indicating the high hardness of this high-pressure carbon allotrope.
High pressure, low temperature Raman measurements performed on LaMnO3 up to 34 GPa provide the first experimental evidence for the persistence of the Jahn-Teller distortion over the entire stability range of the insulating phase. This result resolves the ongoing debate about the nature of the pressure driven insulator to metal transition (IMT), demonstrating that LaMnO3 is not a classical Mott insulator. The formation of domains of distorted and regular octahedra, observed from 3 to 34 GPa, sheds new light on the mechanism behind the IMT suggesting that LaMnO3 becomes metallic when the fraction of undistorted octahedra domains increases beyond a critical threshold.
We report on a Raman-scattering investigation of the charge density wave (CDW), quasi-two-dimensional rare-earth tritellurides RTe(3) (R=La, Ce, Pr, Nd, Sm, Gd, and Dy) at ambient pressure, and of LaTe(3) and CeTe(3) under externally applied pressure. The observed phonon peaks can be ascribed to the Raman-active modes for both the undistorted and the distorted lattices in the CDW state by means of a first-principles calculation. The latter also predicts the Kohn anomaly in the phonon dispersion, driving the CDW transition. The integrated intensity of the two most prominent modes scales as a characteristic power of the CDW-gap amplitude upon compressing the lattice, which provides clear evidence for the tight coupling between the CDW condensate and the vibrational modes
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